Near-unity electrochemical conversion of nitrate to ammonia on crystalline nickel porphyrin-based covalent organic frameworks

Abstract

Electrochemical nitrate reduction can potentially enable the indirect fixation of atmospheric N2, as well as the efficient nitrate removal from industrial wastewater, which has attracted rapidly increasing attention over recent...

Molecular electrocatalysts for rapid and selective reduction of nitrogenous waste to ammonia

“…S9, ESI†). These TOF values are higher than the those of the recently reported NO 3 RR catalysts, such as NiPr-TPA-COF (3.5 s −1 ) 33 and FePPy-SACs (0.7 s −1 ). 6 The EIS spectra show that the CuPc MDE exhibits much smaller electron transfer resistance than that of the CuPc AE, which can explain the higher activity of the CuPc MDE for NH 3 production (Fig.…”

Defect engineering of two-dimensional materials for advanced energy conversion and storage

“…338,350,351 More importantly, the nitrate (NO 3 À ) source is almost ubiquitous in industrial wastewater and polluted groundwater, the sustainable recycling of which is undoubtedly a significant contribution to the regulation of the global nitrogen cycle. 352,353 Specifically, the NO 3 RR pathway (NO 3 À + 6H 2 O + 8e À -NH 3 + 9OH À ) on the electrode surface consists of several steps: adsorption of NO 3 À , deoxygenation followed by hydrogenation of N species, and desorption of the reduced products. Due to the complex multistep reaction and thermodynamic potential (0.69 V) of NO 3 RR versus the reversible hydrogen electrode (RHE), the potential byproducts (e.g., NO 2 , NO, N 2 O, and N 2 ) are formed through undesired pathways and the competitive HER might impair NH 3 conversion efficiency.…”

Synthesis and Design of Hybrid Metalloporphyrin Polymers Based on Palladium (II) and Copper (II) Cations and Axial Complexes of Pyridyl-Substituted Sn(IV)Porphyrins with Octopamine

“…Coordination polymers based on metal complexes of tetrapyrrole macrocyclic compounds represent a special group of self-organized systems that combine their structural fragments through non-covalent interactions [ 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 ]. Such interactions are reversible and easily controlled by various external influences.…”

“…Therefore, the coordination self-assembly is a convenient tool to create stable and controllable architectures by the self-organization of metal and organic components with electronic and geometric complementarity. Different functional substituents, the type of organic fragments binding, the metal nature, and the length of the linking fragments provide a variety of framework structure types and areas of their potential application [ 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 , 29 , 30 , 31 , 32 , 33 , 34 , 35 , 36 , 37 ]. The construction of supramolecular porphyrin scaffolds is still little studied, but it is undoubtedly an urgent scientific problem, the solution of which will to get closer to understanding the life processes of nature.…”